Valence and spin fluctuations in the Mn-doped ferroelectric BaTiO3

Mandal, Subhasish; Cohen, R. E.; Haule, K.

doi:10.1103/PhysRevB.98.075155

Title: Valence and spin fluctuations in the Mn-doped ferroelectric ${BaTiO}_{3}$

Journal Article · Wed Aug 29 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.075155· OSTI ID:1544223

Mandal, Subhasish ^[1]; Cohen, R. E. ^[2]; Haule, K. ^[3]

Yale Univ., New Haven, CT (United States). Dept. of Applied Physics; Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.
Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.; Ludwig Maximilian Univ., Munich (Germany). Dept. of Earth and Environmental Sciences
4Department of Physics, Rutgers University, Piscataway, New Jersey 08854, USA

We study Mn substitution for ${BaTiO}_{3}$ with and without compensating oxygen vacancies using density functional theory (DFT) in combination with dynamical mean-field theory (DMFT). We find strong charge and spin fluctuations. Without compensating oxygen vacancies, the ground state is found to be a quantum superposition of two distinct atomic valences, $3d^4$ and $3d^5$. Introducing a compensating oxygen vacancy at a neighboring site reduces both charge and spin fluctuations due to the reduction of electron hopping from Mn to its ligands. As a consequence, valence fluctuations are reduced, and the valence is closely fixed to the high spin $3d^5$ state. Here we show that inclusion of charge and spin fluctuations is necessary to obtain an accurate ground state of transition metal-doped ferroelectrics.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: N00014-12-1-1038; N00014-14-1-0561; N00014-17-1-2768; ACI-1339804; DMR-1709229

OSTI ID:: 1544223

Journal Information:: Physical Review B, Vol. 98, Issue 7; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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